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US2530367A - Disproportionation of alkoxysilanes - Google Patents

Disproportionation of alkoxysilanes Download PDF

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Publication number
US2530367A
US2530367A US790230A US79023047A US2530367A US 2530367 A US2530367 A US 2530367A US 790230 A US790230 A US 790230A US 79023047 A US79023047 A US 79023047A US 2530367 A US2530367 A US 2530367A
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Prior art keywords
temperature
group
alkoxysilane
silane
silicon
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US790230A
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Charles R Hance
George H Wagner
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Linde Air Products Co
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Linde Air Products Co
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Priority to US790230A priority Critical patent/US2530367A/en
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    • CCHEMISTRY; METALLURGY
    • C01INORGANIC CHEMISTRY
    • C01BNON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B33/00Silicon; Compounds thereof
    • C01B33/04Hydrides of silicon
    • C01B33/043Monosilane
    • CCHEMISTRY; METALLURGY
    • C07ORGANIC CHEMISTRY
    • C07FACYCLIC, CARBOCYCLIC OR HETEROCYCLIC COMPOUNDS CONTAINING ELEMENTS OTHER THAN CARBON, HYDROGEN, HALOGEN, OXYGEN, NITROGEN, SULFUR, SELENIUM OR TELLURIUM
    • C07F7/00Compounds containing elements of Groups 4 or 14 of the Periodic Table
    • C07F7/02Silicon compounds
    • C07F7/04Esters of silicic acids

Definitions

  • the invention is a process for disproportionating alkoxysilanes. It affords a means of effecting, in an assemblage of silicon-containing molecules each comprising at least one hydrogen atom and at least one alkoxy group, a redistribution in such fashion that silicon-containing molecules devoid of alkoxy groups are formed concomitantly with silicon-containing molecules in which no Si-H bond is present.
  • triethoxysilane SiH(OC2H5) 3 a readily available compound, can be caused to undergo the transformation depicted by the equation Valuable products are thereby formed-in this example silane and tetraethylorthosilicate.
  • the disproportionation is carried out by treating the allroxysilane with a suitable catalyst at an appropriate temperature.
  • a suitable catalyst we prefer a compound of the type represented by the formula MOE, where M is a metal of group IA of the periodic table, and R is hydrogen or an alkyl group.
  • MOE metal of group IA of the periodic table
  • R is hydrogen or an alkyl group.
  • the hydroxides and ethoxides of sodium and potassium are preferred.
  • the quantity of catalyst used is not critical, and since the preferred catalysts are inexpensive substances, 0.5 or more has been used in most of our tests.
  • the temperature employed may range from room temperature or below to moderate heating, for example to 60 C. Raising the temperature accelerates the reaction but may reduce the chiciency, as by causing hydrogen to appear in considerable proportions in the gaseous product. Even at room temperatures the velocity of the reaction is such as to be adequate in many cases.
  • silane when 0.65% of NaOCzHa was added to 7.5 g. of SiI-I(OC2H5)3 at 26 0., silane was evolved at the rate of 3.3 cc. per minute; at 40 C. the rate increased to 4.4 cc./min., and at 60 C. to 8/1 cc./min. Increasing the proportion of ethoxide catalyst to 2.1% gave 20.7 cc./min. of silane at 26 C.
  • the hydroxides show activity of the same order as the ethoxides. If a very rapid evolution of gas is desired, as in some prospective applications of the invention, either the proportion of catalyst or the temperature or both are increased.
  • ThllSfWith 1 of NaOH at 60 C. silane (containing some 30% of Hz) was evolved at the rate of more than 50 cc./min. from a 7.5 g. sample of SiH(OC2I-I5)3.
  • Process of disproportionating an alkoxysilane containing at least one hydrogen atom at tached to silicon which comprises treating said alkoxysilane, at a temperature not substantially above about C., with a compound in solid form having the type formula MOR, Where M is a metal of group IA of the periodic table, and R is a member of the group consisting of hydrogen and alkyl radicals, and recovering silane from the reaction product.
  • Process of disproportionating an alkoxysilane containing at least one hydrogen atom attached to silicon which comprises treating said alkoxysilane, at a temperature not substantially above about 60 C., with a solid alkali metal alkoxide, and recovering silane from the reaction product.
  • Process of disproportionating an alkoxysilane containing at least one hydrogen atom attached to silicon which comprises treating said alkoxysilane, at a temperature not substantially above about 60 C., with a solid alkali metal hydroxide, and recovering silane from the reaction product.
  • Process of disproportionating a trialkoxysilane which comprises treating it, at a temperature not substantially above about 60 C., with a solid alkali metal alkoxide, and recovering silane from the reaction product.

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  • Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Inorganic Chemistry (AREA)

Description

Patented Nov. 21, 1950 DISPROPORTIONATION OF ALKOXYSILANES Charles R. Hance, Durham, N. 0., and George H. Wagner, Kenmore, N. Y., assignors to The Linde Air Products Company, a corporation of Ohio No Drawing. Application December 6, 1947, Serial No. 790,230
Claims.
The invention is a process for disproportionating alkoxysilanes. It affords a means of effecting, in an assemblage of silicon-containing molecules each comprising at least one hydrogen atom and at least one alkoxy group, a redistribution in such fashion that silicon-containing molecules devoid of alkoxy groups are formed concomitantly with silicon-containing molecules in which no Si-H bond is present. Thus, triethoxysilane SiH(OC2H5) 3 a readily available compound, can be caused to undergo the transformation depicted by the equation Valuable products are thereby formed-in this example silane and tetraethylorthosilicate.
The disproportionation is carried out by treating the allroxysilane with a suitable catalyst at an appropriate temperature. For the catalyst we prefer a compound of the type represented by the formula MOE, where M is a metal of group IA of the periodic table, and R is hydrogen or an alkyl group. The hydroxides and ethoxides of sodium and potassium are preferred. The quantity of catalyst used is not critical, and since the preferred catalysts are inexpensive substances, 0.5 or more has been used in most of our tests.
The temperature employed may range from room temperature or below to moderate heating, for example to 60 C. Raising the temperature accelerates the reaction but may reduce the chiciency, as by causing hydrogen to appear in considerable proportions in the gaseous product. Even at room temperatures the velocity of the reaction is such as to be adequate in many cases. Thus, when 0.65% of NaOCzHa was added to 7.5 g. of SiI-I(OC2H5)3 at 26 0., silane Was evolved at the rate of 3.3 cc. per minute; at 40 C. the rate increased to 4.4 cc./min., and at 60 C. to 8/1 cc./min. Increasing the proportion of ethoxide catalyst to 2.1% gave 20.7 cc./min. of silane at 26 C. The hydroxides show activity of the same order as the ethoxides. If a very rapid evolution of gas is desired, as in some prospective applications of the invention, either the proportion of catalyst or the temperature or both are increased. ThllSfWith 1 of NaOH at 60 C. silane (containing some 30% of Hz) was evolved at the rate of more than 50 cc./min. from a 7.5 g. sample of SiH(OC2I-I5)3.
What is claimed is:
1. Process of disproportionating an alkoxysilane containing at least one hydrogen atom at tached to silicon, which comprises treating said alkoxysilane, at a temperature not substantially above about C., with a compound in solid form having the type formula MOR, Where M is a metal of group IA of the periodic table, and R is a member of the group consisting of hydrogen and alkyl radicals, and recovering silane from the reaction product.
2. Process of disproportionating an alkoxysilane containing at least one hydrogen atom attached to silicon, which comprises treating said alkoxysilane, at a temperature not substantially above about 60 C., with a solid alkali metal alkoxide, and recovering silane from the reaction product.
3. Process of disproportionating an alkoxysilane containing at least one hydrogen atom attached to silicon, which comprises treating said alkoxysilane, at a temperature not substantially above about 60 C., with a solid alkali metal hydroxide, and recovering silane from the reaction product.
4. Process of disproportionating a trialkoxysilane which comprises treating it, at a temperature not substantially above about 60 C., with a solid alkali metal alkoxide, and recovering silane from the reaction product.
5. Process of disproportionating triethoXysilane which comprises treating it, at a temperature not substantially above about 60 C., with a compound in solid form having the type formula MOR, Where M is a metal of group IA of the periodic table, and R is a member of the group consisting of hydrogen and alkyl radicals, and recovering silane from the reaction product.
CHARLES R. HANCE. GEORGE H. WAGNER.
REFERENCES CITED The following references are of record in the file of this patent:
Friedel: Annalen der Chemie, vol. 143. (1867) pages 124-127.
Taurke: Berichte, vol. 38 (1905) pages 1661, 1662.
Post: The Chemistry of Aliphatic Ortho Esters, page 146, 147. Published by Reinhold. N. Y., 1943.

Claims (1)

1. PROCESS OF DISPORPORTIONATING AN ALKOXYSILANE CONTAINING AT LEAST ONE HYDROGEN ATOM ATTACHED TO SILICON, WHICH COMPRISES TREATING SAID ALKOXYSILANE, AT A TEMPERATURE NOT SUBSTANTAILLY ABOVE ABOUT 60*C., WITH A COMPOUND IN SOLID FORM HAVING THE TYPE FORMULA MOR, WHERE M IS A METAL OF GROUP IA OF THE PERIODIC TABLE, AND R IS A MEMBER OF THE GROUP CONSISTING OF HYDROGEN AND ALKYL RADICALS, AND RECOVERING SILANE FROM THE REACTION PRODUCT.
US790230A 1947-12-06 1947-12-06 Disproportionation of alkoxysilanes Expired - Lifetime US2530367A (en)

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Cited By (12)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US2723985A (en) * 1952-10-17 1955-11-15 Union Carbide & Carbon Corp Disproportionation of allyl- and butenylalkoxysilanes
US2723983A (en) * 1952-10-16 1955-11-15 Union Carbide & Carbon Corp Disproportionation of hydrocarbon alkoxysilanes
US2723984A (en) * 1952-10-17 1955-11-15 Union Carbide & Carbon Corp Disproportionation of arylalkoxysilanes
US2735861A (en) * 1956-02-21 Disproportionation of alkoxy silane
US2745860A (en) * 1952-10-16 1956-05-15 Union Carbide & Carbon Corp Disproportionation of alkoxydisilyl hydrocarbons
US3463660A (en) * 1965-05-11 1969-08-26 Ici Ltd Process for obtaining an anti-stick surface with an organosilicon and an organopolysiloxane and a cooking utensil so treated
DE2247873A1 (en) * 1971-10-01 1973-04-05 Tokyo Shibaura Electric Co PROCESS FOR THE PRODUCTION OF SILANES
EP0337322A3 (en) * 1988-04-13 1991-03-27 Mitsubishi Kasei Corporation Process for producing monosilane
US5126472A (en) * 1991-11-12 1992-06-30 Dow Corning Corporation Thermal disproportionation of organooxysilanes
US5126471A (en) * 1991-11-14 1992-06-30 Dow Corning Corporation Thermal disproportionation of cycloalkylsilanes
RU2279403C1 (en) * 2004-12-27 2006-07-10 Федеральное государственное унитарное предприятие "Государственный научно-исследовательский институт химии и технологии элементоорганических соединений" (ФГУП ГНИИХТЭОС) High-purity monosilane production process
WO2014054889A1 (en) 2012-10-02 2014-04-10 오씨아이 주식회사 Method for preparing monosilane using trialkoxysilane

Non-Patent Citations (1)

* Cited by examiner, † Cited by third party
Title
None *

Cited By (14)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US2735861A (en) * 1956-02-21 Disproportionation of alkoxy silane
US2723983A (en) * 1952-10-16 1955-11-15 Union Carbide & Carbon Corp Disproportionation of hydrocarbon alkoxysilanes
US2745860A (en) * 1952-10-16 1956-05-15 Union Carbide & Carbon Corp Disproportionation of alkoxydisilyl hydrocarbons
US2723985A (en) * 1952-10-17 1955-11-15 Union Carbide & Carbon Corp Disproportionation of allyl- and butenylalkoxysilanes
US2723984A (en) * 1952-10-17 1955-11-15 Union Carbide & Carbon Corp Disproportionation of arylalkoxysilanes
US3463660A (en) * 1965-05-11 1969-08-26 Ici Ltd Process for obtaining an anti-stick surface with an organosilicon and an organopolysiloxane and a cooking utensil so treated
DE2247873A1 (en) * 1971-10-01 1973-04-05 Tokyo Shibaura Electric Co PROCESS FOR THE PRODUCTION OF SILANES
EP0337322A3 (en) * 1988-04-13 1991-03-27 Mitsubishi Kasei Corporation Process for producing monosilane
US5126472A (en) * 1991-11-12 1992-06-30 Dow Corning Corporation Thermal disproportionation of organooxysilanes
EP0542243A1 (en) * 1991-11-12 1993-05-19 Dow Corning Corporation Thermal disproportionation of organooxysilanes
US5126471A (en) * 1991-11-14 1992-06-30 Dow Corning Corporation Thermal disproportionation of cycloalkylsilanes
RU2279403C1 (en) * 2004-12-27 2006-07-10 Федеральное государственное унитарное предприятие "Государственный научно-исследовательский институт химии и технологии элементоорганических соединений" (ФГУП ГНИИХТЭОС) High-purity monosilane production process
WO2014054889A1 (en) 2012-10-02 2014-04-10 오씨아이 주식회사 Method for preparing monosilane using trialkoxysilane
US9278864B2 (en) 2012-10-02 2016-03-08 Oci Company Ltd. Method for preparing monosilane using trialkoxysilane

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